The observation of any atomic and molecular dynamics requires a probe that has a timescale comparable to the dynamics itself. Ever since the invention of laser, the temporal duration of the laser pulse has been incrementally reduced from several nanoseconds to just attoseconds. Picosecond and femtosecond laser pulses have been widely used to study molecular rotation and vibration. In 2001, the first single isolated attosecond pulse (1 attosecond = 10^-18 seconds.) was demonstrated. Since this breakthrough, "attoscience" has become a hot topic in ultrafast physics. Attosecond pulses typically have span between EUV to X-ray photon energies and sub-femtosecond pulse duration. It becomes an ideal tool for experimentalists to study ultrafast electron dynamics in atoms, molecules and condensed matter. The conventional scheme for generating attosecond pulses is focusing an intense femtosecond laser pulse into inert gases. The bound electrons are ionized into continuum through tunneling ionization under the strong electrical field. After ionization, the free electron will be accelerated by the laser field away from the parent ion and then recombined with its parent ion and releases its kinetic energy as a photon burst that lasts for a few hundred attoseconds. According to the classical "three-step model", high order harmonic will have a higher cutoff photon energy when driven by a longer wavelength laser field. Compared to Ti:sapphire lasers center at a wavelength of 800 nm, an optical parametric amplifier could offer a broad bandwidth at infrared range, which could support few cycle pulses for driving high harmonic generation in the X-ray spectrum range. In this work, an optical parametric chirped-pulse amplification system was developed to deliver CEP-stable 3-mJ, 12-fs pulses centered at 1.7 micron. We implement a chirped-pump technique to phase match the board parametric amplification bandwidth with high conversion efficiency. Using such a laser source, isolated attosecond pulses with photon exceeding 300 eV are achieved by applying the polarization gating technique at 1.7 micron. The intrinsic positive chirp of the attosecond pulses is measured by the attosecond streak camera and retrieved with our PROOF technique. Sn metal filters with negative dispersion were chosen to compensate the intrinsic attochirp. As a result, isolated 53-attosecond soft x-ray pulses are achieved. Such water window attosecond source will be a powerful tool for studying charge distribution/migration in bio-molecules and will bring opportunities to study high field physics or attochemistry.


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Graduation Date





Chang, Zenghu


Doctor of Philosophy (Ph.D.)


College of Optics and Photonics


Optics and Photonics

Degree Program

Optics and Photonics









Release Date

May 2018

Length of Campus-only Access


Access Status

Doctoral Dissertation (Open Access)